CN101935566B - Biological combined desulfurization method and device for natural gas - Google Patents
Biological combined desulfurization method and device for natural gas Download PDFInfo
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- CN101935566B CN101935566B CN2010102850426A CN201010285042A CN101935566B CN 101935566 B CN101935566 B CN 101935566B CN 2010102850426 A CN2010102850426 A CN 2010102850426A CN 201010285042 A CN201010285042 A CN 201010285042A CN 101935566 B CN101935566 B CN 101935566B
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Abstract
The invention discloses a biological combined desulfurization method and a biological combined desulfurization device for a natural gas, which belong to the field of the application energy source of natural gas and are mainly applied to the removal of sulfur from the natural gas. Through the method and the device, hydrogen sulfide, and the organic sulfur of carbonyl sulfide, sulfur alcohol and the like can be simultaneously removed by microbial action, wherein the hydrogen sulfide is removed by regenerating absorption solution by using microorganisms, while the organic sulfur is removed directly by automatically-separated desulfurization bacteria. The desulfurization device comprises a hydrogen sulfide absorption tower, a biological regeneration tower, a biological trickling filtration tower for removing the organic sulfur, a precipitation tank and the like. The natural gas enters from a gas inlet at the bottom of the hydrogen sulfur absorption tower, is discharged from the top after being reacted, and enters the biological trickling filtration tower for removing the organic sulfur; and then the hydrogen sulfur and the organic sulfur are removed in two reactors respectively. The absorption solution reacted in the hydrogen sulfur absorption tower is precipitated in the precipitation tank, enters the regeneration tower for regeneration and then flows back to the hydrogen sulfur absorption tower for recycling. The method has the advantages of capability of ensuring the continuous and stable removal of the hydrogen sulfur and removing a part of organic sulfur, and lower cost and no secondary pollution compared with physicochemical methods.
Description
Technical field
The invention belongs to the application energy---the Sweet natural gas field, specifically a kind of biological combined desulfurization method of Sweet natural gas is applied to the purification of Sweet natural gas, can effectively remove hydrogen sulfide and organosulfur in the Sweet natural gas simultaneously.
Background technology
The organosulfur compound such as hydrogen sulfide, carbonylsulfide, dithiocarbonic anhydride, mercaptan, thioether that contains high-content in the Sweet natural gas that the most area is verified.Be up to 17% such as content in the Sweet natural gas of verifying in the Northeast, river, total organic sulfur content of some gas well has reached 557.7mg/m
3(Hu Tianyou, seal is respected.The research of high sulfur-containing natural gas organic sulfur removal technology.The oil and gas chemical industry, 2007,36(6) 470-474).These sulphur compounds not only can reduce the thermal capacitance of Sweet natural gas but also poisonous, contaminate environment, and being harmful to health also has powerful corrodibility, so must carry out desulfurization in the use of Sweet natural gas or before carrying.
Method for the selexol process comparative maturity generally can be divided into wet desulphurization and dry desulfurization.Wet desulphurization mainly comprises the chemical solvents method, physical solvent process and mixed solvent method, and wherein the amine absorption process application is the most ripe at most, but it exists equipment huge, and the investment working cost is high, the problems such as regeneration difficulty and environmental pollution.Dry desulfurization also exists desulfurizer regeneration suffering or non-renewable, high in cost of production problem.It is the new technology of development in recent years that Natural Gas Membrane separates desulfurization, has overcome the deficiency that many tradition purify.Such as Chinese patent application CN 1785480A " membrane adsorption natural gas desulfur method ", utilize membrane absorption method to remove hydrogen sulfide in the Sweet natural gas, the gases such as organosulfur.The method is used the sulphur in the microporous hollow fiber separating natural gas, oozes out again after sulfur is absorbed by liquid absorption to be collected in revivifier from absorption liquid, and absorption liquid returns to and carries out recycle.Though the method has been utilized the film of less energy-consumption, but hydro carbons oozes out the greater loss that can cause energy in the process.
Than above method, the biological desulphurization method possesses the advantages such as cost low reaction mild condition, less energy consumption, effective environmental contamination reduction.Arranged larger development prospect.
Summary of the invention
The object of the present invention is to provide a kind of biological desulfurization method of Sweet natural gas, this method not only can remove hydrogen sulfide can also remove organosulfur, can stablize to generate simple substance S the renewable rear recycling of absorption liquid, device continuously-running in the reaction of hydrogen sulfide.Whole technology investment running cost is low, non-secondary pollution.
The present invention adopts following technical scheme:
A kind of biological process Sweet natural gas combination sulfur removal technology, it adds microorganism to the regeneration of molysite take iron salt oxidization hydrogen sulfide method as the basis, desulfurization bacterium consists of its primary structure to the removal of organosulfur.Sweet natural gas is removed hydrogen sulfide and is become elemental sulfur through the oxygenizement of iron salt solutions first, carries out the removal of organosulfur through the effect of desulfurization microorganism again.Reacted iron salt solutions carries out after the separation of simple substance S the again effect of microorganism regenerates, and then carries out recycle.The nutritive medium that removal of organic sulfur from partly sprays acts in tower by after reconcile replenishing and recycling.
Whole reaction process only in the bio-regeneration tower aeration microorganism is had an effect.Two reactors of ventilation body: hydrogen sulfide absorption tower and organosulfur bio-trickling filter are all without external aeration.
Relevant reaction is as follows:
The hydrogen sulfide absorption stage: H
2S+Fe
2(SO
4)
3→ S+ 2FeSO
4+ H
2SO
4
The regeneration of absorption solution stage: FeSO
4+ H
2SO
4+ 1/2O
2→ Fe
2(SO
4)
3+ H
2O
The bio-trickling filter bio-oxidation stage: CH
3SH+3.5O
2→ CO
2+ H
2O+H
2SO
4
CS
2+H
2O?→COS+H
2S
COS+H
2S+O
2?→CO
2+H
2SO
4
Concrete sulfur method of the present invention is as follows:
First paragraph is for removing hydrogen sulfide: with the iron salt solutions that contains microorganism that in the bio-regeneration tower, reacted in advance as the absorption liquid in the hydrogen sulfide absorption tower, allow the inlet mouth of Sweet natural gas at the bottom of the hydrogen sulfide absorption tower enter, contact with absorption liquid in the hydrogen sulfide absorption tower, hydrogen sulfide wherein is oxidized to simple substance S; Reacted absorption liquid flows into settling bath from the liquid outlet of bottom, absorption tower, and simple substance S is separated in settling bath; Absorption liquid after separating enters the bio-regeneration tower, and the filler in the bio-regeneration tower is gac, is loaded with the bacterium that ferrous Quick Oxidation can be become high ferro on the filler, and the absorption liquid after the regeneration is got back to the utilization of hydrogen sulfide absorption tower internal recycle again through recycle pump;
Second segment is for removing organosulfur: the Sweet natural gas through preliminary treatment is discharged the inlet mouth that enters the bio-trickling tower bottom from the air outlet of hydrogen sulfide absorption tower upper end, the bio-trickling inner-tower filling material is the light ceramic that is loaded with desulfurization bacterium, gas passes through filler, with microbial process in the filler and with reverse contact of spray liquid that flows down from dripping filter tower top spray nozzle, the organosulfurs such as mercaptan wherein, dithiocarbonic anhydride, carbonylsulfide are partly removed, and discharge from total air outlet through the Sweet natural gas of double diffusion; Leakage fluid dram from the bio-trickling filter below after spray liquid contacts with gas, filler enters reservoir, gets to the bio-trickling filter top through recycle pump again and carries out recycle;
Device needs after operation for some time to replenish the part spray liquid in reservoir, regulates pH to initial value.
The desulfurizer that the present invention adopts is as follows:
Device comprises hydrogen sulfide absorption tower, bio-regeneration tower, bio-trickling filter and settling bath;
Be provided with Sweet natural gas inlet mouth, liquid outlet at described hydrogen sulfide absorption tower bottom, top sets out gas port and fluid inlet, and described air outlet links to each other with the inlet mouth of the bio-trickling tower bottom of removal of organic sulfur from, and Sweet natural gas carries out removing of hydrogen sulfide in this tower;
The liquid outlet of described hydrogen sulfide absorption tower is connected with the settling bath fluid inlet, and the liquid outlet of settling bath links to each other with the fluid inlet of bio-regeneration tower bottom; Establish packing layer in the described bio-regeneration tower, be loaded with the bacterium that ferrous Quick Oxidation can be become high ferro on the filler, the absorption liquid after the regeneration carries out recycle from the liquid outlet of bio-regeneration tower upper end by the fluid inlet that recycle pump enters hydrogen sulfide absorption tower upper end;
In the described bio-trickling filter take the light ceramic that is loaded with desulfurization bacterium as filler, the top of bio-trickling filter is provided with mouth spray and total air outlet, by the gas spray spray liquid of mouth spray to the filler of flowing through, the processing of removing organosulfur is discharged from total air outlet through the Sweet natural gas of double diffusion; The bio-trickling filter below is provided with leakage fluid dram and discharges spray liquid, connects reservoir, and the spray liquid in the reservoir is the mouth spray through recycle pump is connected to bio-trickling filter by pipeline above again, carries out recycle.
Beneficial effect of the present invention is:
1. by two large segment process, remove most hydrogen sulfide and part organosulfur in the Sweet natural gas, realized jointly removing of inorganic sulfur and organosulfur.
2. in the removal part of hydrogen sulfide: use molysite to absorb, hydrogen sulfide is oxidized to simple substance S, precipitate and separate in settling bath.Reacted absorption liquid returns the absorption tower recycle after entering regenerator column regeneration.Namely do not have secondary pollution to accomplish again the recycle of absorption liquid, and by to the adjusting of parameter between absorption tower and regenerator column, can reach and run without interruption.
3. in the removal part of organosulfur: adopt and drip a filter tower, spray liquid gets off contact with filler afterwards and enters circulation groove from the bottom liquid outlet and get to the top through water circulating pump again and spray from dripping a filter tower top spray.Replenish again suitable spray liquid after the long-time running and regulate pH to initial value.Drip microorganism in the filter tower filler and be from being separated for a long time acquisition thiophene, the dithiocarbonic anhydride contaminated soil, under the condition of imposed aeration not, also can have an effect, can remove the organosulfurs such as mercaptan, dithiocarbonic anhydride, carbonylsulfide.
Description of drawings
Fig. 1 is the synoptic diagram of the life assemblage desulfurizer of Sweet natural gas of the present invention.
1. hydrogen sulfide absorption tower; 2. bio-regeneration tower; 3. bio-trickling filter; 4. settling bath; 5. reservoir; 6. recycle pump; 7. aeration pump; 8. Sweet natural gas inlet mouth; 9. air outlet, absorption tower; 10. drip the filter tower inlet mouth; 11. total air outlet; 12. absorption liquid leakage fluid dram; 13. settling bath fluid inlet; 14. settling bath leakage fluid dram; 15. regenerator column fluid inlet; 16. communicating pipe; 17. circulation fluid fluid inlet; 18. drip the filtrate leakage fluid dram; 19. mouth spray; 20. ceramics filling; 21. water distribution board; 22. active carbon filler.
Embodiment
Below by specific embodiment the present invention is described in further detail, to help understanding content of the present invention.
As shown in Figure 1, the absorption liquid in the hydrogen sulfide absorption tower 1 is at the complete iron salt solutions that contains microorganism of bio-regeneration tower 2 interior prior reactions.The Sweet natural gas inlet mouth 8 of Sweet natural gas at the bottom of the hydrogen sulfide absorption tower enters, and contacts with absorption liquid in hydrogen sulfide absorption tower 1, and hydrogen sulfide wherein is oxidized to simple substance S.Reacted absorption liquid flows into settling bath 4 from the absorption liquid leakage fluid dram 12 of hydrogen sulfide absorption tower 1 bottom, and simple substance S is separated in settling bath 4.Absorption liquid after separating enters bio-regeneration tower 2, and the filler 22 in the bio-regeneration tower 2 is gac, is loaded with the bacterium that ferrous Quick Oxidation can be become high ferro on the filler, and the absorption liquid after the regeneration is got back to the 1 internal recycle utilization of hydrogen sulfide absorption tower again through recycle pump 6.Below just finished removing hydrogen sulfide.
The Sweet natural gas of preliminary treatment is discharged the titration tower inlet mouth 10 that enters bio-trickling filter 1 bottom from the air outlet, absorption tower 9 of hydrogen sulfide absorption tower 2 upper ends, filler 20 in the bio-trickling filter 1 is for being loaded with the light ceramic of desulfurization bacterium, gas is by being loaded with the filler of desulfurization bacterium, with microbial process in the filler 20 and reverse contact of spray liquid that flow down with mouth spray 19 from bio-trickling filter 1 top, the organosulfurs such as mercaptan wherein, dithiocarbonic anhydride, carbonylsulfide are partly removed, and discharge from total air outlet 11 through the Sweet natural gas of double diffusion.Titration tower leakage fluid dram 18 from bio-trickling filter 1 below after spray liquid contacts with gas, filler enters reservoir 5, gets to the bio-trickling filter top through recycle pump 6 ' again and carries out recycle.Need after operation for some time in reservoir 5, to replenish the part spray liquid, regulate pH to initial value.
Wherein, the bacterium in the regeneration of absorption solution tower packing is adopted the chemoautotrophic bacteria thiobacillus ferrooxidant, plays oxygenizement, makes the absorption liquid recycle.
The desulfurization bacterium that is loaded with in the bio-trickling tower packing preferably adopts the microbacterium mixed bacterial, and described microbacterium mixed bacterial obtains by the method separation and Culture:
(1) sampling is certainly for a long time through thiophene and dithiocarbonic anhydride contaminated soil;
(2) substratum of separation organosulfur: minimum medium BSM consists of K
2HPO
43H
2O 5.0 g, NaH
2PO
42H
2O 2.0 g, MgCl
26H
2O 0.2 g, NH
4Cl 2.0g, glycerine 2 g, micro-1 mL, distilled water 1000 mL; Trace element consists of CuCl
22H
2O 0.1g, COCl
26H
2O 0.4g, ZnCl
20.2g, CaCl
20.2g, H
3BO
30.05g, NaMoO
42H
2O 0.2g, FeCl
37H
2O 0.1g, AlCl
36H
2O 0.1g, MnCl
24H
2O 0.4 g/L;
The sulphur source is 0.2mmol/L sulfur alcohol or dithiocarbonic anhydride;
Continuous enrichment culture is isolated two strain bacterium DOS-1, DOS-2 under (3) 30 ℃ of conditions, all belongs to Microbacterium through Physiology and biochemistry and 16srDNA evaluation, and the peculiar bacterium of genusization energy is good foster, weak anaerobism, 30 ℃ of optimum growth temperatures.
Spray liquid is the mixed solution dipotassium hydrogen phosphate 5.0g/L of following component, SODIUM PHOSPHATE, MONOBASIC 2.0g/L, magnesium chloride 0.2g/L, ammonium chloride 2.0g/L, glycerine 2g/L, cupric chloride 0.1g/L, calcium chloride 0.05g/L, Sodium orthomolybdate 0.2g/L, iron(ic) chloride 0.1g/L, Manganous chloride tetrahydrate 0.4g/L, zinc chloride 0.2g/L, pH=7.
Claims (4)
1. the biological combined desulfurization method of Sweet natural gas, the hydrogen sulfide absorption tower that described method adopts, bio-regeneration tower, removal of organic sulfur from bio-trickling filter and settling bath form desulfurizer, use two stage process that hydrogen sulfide in natural gas and organosulfur are removed respectively;
First paragraph is for removing hydrogen sulfide: with the prior iron salt solutions that contains microorganism that has reacted bio-regeneration tower (2) in as the absorption liquid in the hydrogen sulfide absorption tower (1), allow the inlet mouth (8) of Sweet natural gas at the bottom of the hydrogen sulfide absorption tower enter, contact with absorption liquid in the hydrogen sulfide absorption tower, hydrogen sulfide wherein is oxidized to simple substance S; Reacted absorption liquid flows into settling bath (4) from the liquid outlet (12) of bottom, absorption tower, and simple substance S is separated in settling bath (4); Absorption liquid after separating enters bio-regeneration tower (2), filler (22) in the bio-regeneration tower (2) is gac, be loaded with the bacterium that ferrous Quick Oxidation can be become high ferro on the filler, the absorption liquid after the regeneration is got back to hydrogen sulfide absorption tower (1) internal recycle utilization again through the first recycle pump (6);
Second segment is for removing organosulfur: will discharge the inlet mouth (10) that enters bio-trickling filter (3) bottom from the air outlet (9) of hydrogen sulfide absorption tower (1) upper end through the Sweet natural gas of preliminary treatment, bio-trickling inner-tower filling material (20) is for being loaded with the light ceramic of desulfurization bacterium, gas passes through filler, with microbial process in the filler and with reverse contact of spray liquid that flows down from dripping filter tower top spray nozzle (19), the organosulfurs such as mercaptan wherein, dithiocarbonic anhydride, carbonylsulfide are partly removed, and discharge from total air outlet (11) through the Sweet natural gas of double diffusion; Leakage fluid dram (18) from bio-trickling filter (3) below after spray liquid contacts with gas, filler enters reservoir (5), gets to bio-trickling filter (3) top through the second recycle pump (6 ') again and carries out recycle;
Device needs after operation for some time to add the part spray liquid in reservoir (5), regulates pH to initial value 7.
2. Sweet natural gas biological combined desulfurization method according to claim 1, it is characterized in that: described spray liquid is the mixed solution of following component: dipotassium hydrogen phosphate 5.0g/L, SODIUM PHOSPHATE, MONOBASIC 2.0g/L, magnesium chloride 0.2g/L, ammonium chloride 2.0g/L, glycerine 2g/L, cupric chloride 0.1g/L, calcium chloride 0.05g/L, Sodium orthomolybdate 0.2g/L, iron(ic) chloride 0.1g/L, Manganous chloride tetrahydrate 0.4g/L, zinc chloride 0.2g/L, pH=7.
3. according to the biological combined desulfurization method of right 2 described Sweet natural gases, it is characterized in that: in the hydrogen sulfide absorption tower that leads to Sweet natural gas and removal of organic sulfur from bio-trickling filter, do not need imposed aeration.
4. life assemblage desulfurizer of realizing the Sweet natural gas of claim 1,2 or 3 described methods, it is characterized in that: described device comprises hydrogen sulfide absorption tower (1), bio-regeneration tower (2), bio-trickling filter (3) and settling bath (4), uses two stage process that hydrogen sulfide in natural gas and organosulfur are removed respectively;
Be provided with Sweet natural gas inlet mouth (8), liquid outlet (12) in described hydrogen sulfide absorption tower (1) bottom, top sets out gas port (9) and fluid inlet (17), described air outlet (9) links to each other with the inlet mouth (10) of bio-trickling filter (3) bottom of removal of organic sulfur from, and Sweet natural gas carries out removing of hydrogen sulfide in this tower;
The liquid outlet of described hydrogen sulfide absorption tower (12) is connected with settling bath fluid inlet (13), and the liquid outlet (14) of settling bath (4) links to each other with the fluid inlet (15) of bio-regeneration tower (2) bottom; Establish packing layer in the described bio-regeneration tower (2), be loaded with the bacterium that ferrous Quick Oxidation can be become high ferro on the filler, the absorption liquid after the regeneration carries out recycle from the liquid outlet (16) of bio-regeneration tower (2) upper end by the fluid inlet (17) that the first recycle pump (6) enters hydrogen sulfide absorption tower (1) upper end;
In the described bio-trickling filter take the light ceramic that is loaded with desulfurization bacterium as filler (20), the top of bio-trickling filter (3) is provided with mouth spray (19) and total air outlet, by the gas spray spray liquid of mouth spray (19) to the filler of flowing through, remove the processing of organosulfur, discharge from total air outlet (11) through the Sweet natural gas of double diffusion; Bio-trickling filter (3) below is provided with leakage fluid dram (18) and discharges spray liquid, connect reservoir (5), spray liquid in the reservoir (5) is the mouth spray (19) through the second recycle pump (6 ') is connected to bio-trickling filter (3) by pipeline above again, carries out recycle.
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| CN2010102850426A CN101935566B (en) | 2010-09-17 | 2010-09-17 | Biological combined desulfurization method and device for natural gas |
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| TWI454304B (en) * | 2012-10-08 | 2014-10-01 | Univ Nat Chiao Tung | High concentration h2s elimination system and method |
| CN103071378B (en) * | 2013-01-11 | 2015-07-01 | 中国科学院广州能源研究所 | Two-stage biological desulfuration device of marsh gas |
| CN103585870A (en) * | 2013-10-15 | 2014-02-19 | 天津理工大学 | Method for biologically removing hydrogen sulfide and ammonia gas by steel sulfuric acid pickling waste liquor |
| CN106310890B (en) * | 2015-06-17 | 2019-06-04 | 中国石油化工股份有限公司 | A kind of method of bioanalysis removing sour gas |
| CN106268291A (en) * | 2016-11-03 | 2017-01-04 | 南京工业大学 | Filter tower device and the method for biological desulphurization deodorization are dripped in a kind of biological desulphurization deodorization |
| CN107557089A (en) * | 2017-10-11 | 2018-01-09 | 南京元凯生物能源环保工程有限公司 | A kind of biological desulfurization process for biogas |
| CN109966883A (en) * | 2019-04-25 | 2019-07-05 | 常州南大常高新环保产业技术研究院有限公司 | A kind of biological desulphurization system that internal oxygenating is combined with external oxygenating |
| CN114849462A (en) * | 2021-02-03 | 2022-08-05 | 财团法人工业技术研究院 | Biological desulfurization treatment method and biological desulfurization treatment system |
| CN114181749B (en) * | 2021-12-27 | 2022-09-20 | 华夏碧水环保科技股份有限公司 | Two-section type biogas biological desulfurization device |
Citations (3)
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| US5002888A (en) * | 1990-01-05 | 1991-03-26 | Institute Of Gas Technology | Mutant microorganisms useful for cleavage of organic C-S bonds |
| CN2710731Y (en) * | 2004-07-13 | 2005-07-20 | 徐晓军 | Biological catalystic-oxidation equipment for removing sulphur |
| CN101053765A (en) * | 2007-02-14 | 2007-10-17 | 杭州能源环境工程有限公司 | Sewage biological desulphurizing device |
-
2010
- 2010-09-17 CN CN2010102850426A patent/CN101935566B/en not_active Expired - Fee Related
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5002888A (en) * | 1990-01-05 | 1991-03-26 | Institute Of Gas Technology | Mutant microorganisms useful for cleavage of organic C-S bonds |
| CN2710731Y (en) * | 2004-07-13 | 2005-07-20 | 徐晓军 | Biological catalystic-oxidation equipment for removing sulphur |
| CN101053765A (en) * | 2007-02-14 | 2007-10-17 | 杭州能源环境工程有限公司 | Sewage biological desulphurizing device |
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